Retrieval of microphysical properties of desert dust and volcanic ash aerosols from ground-based remote sensing

Aerosol particles are important constituents of the Earth's atmosphere. To quantify effects of aerosol particles, their distribution and properties need to be known. An important tool for the provision of such information is remote sensing. This thesis covers vertically-resolving remote sensing by lidar and vertically-integrating remote sensing by photometer, and thereby considers desert dust aerosols which cause a major uncertainty in climate forecasts, as well as volcanic ash aerosols which, in addition, are relevant for the flight safety of jet-driven aircrafts. Both aerosol types consist of ensembles of particles of varying size, shape, and chemical composition. This thesis aims to improve the retrieval of the physical properties of such mixtures from remote sensing observations, in particular by using Bayesian approaches and improved aerosol models. Three types of retrievals were developed. The first retrieval type applies to lidar observations, assumes spheroidal particle shapes, and is based on a Bayesian Monte-Carlo-approach. It was applied to observations of a pure volcanic ash plume from Iceland on 17 April 2010 over Maisach (Germany) for the retrieval of the mass concentration of the ash particles. The second retrieval type applies to photometer observations in the solar aureole, uses a pre-defined set of ensembles of irregularly-shaped particles, and was applied to observations of the same ash plume. Both methods consistently retrieved a maximum ash mass concentration of about 1.1 milligram per cubic meter over Maisach with an uncertainty range from 0.7 to 1.5 milligram per cubic meter. The third retrieval type searches for ensembles that agree with the observations from both remote sensing techniques; it uses a pre-defined set of ensembles derived from the aerosol database OPAC, but consisting of absorbing and non-absorbing irregularly-shaped particles. This approach was successfully applied to Saharan dust observations, which were performed during the SAMUM field campaigns in Morocco and on the Cape Verde islands. It turned out that, besides the particle shape, also the presence of non-absorbing components strongly influences the backscattering properties of the aerosols. In contrast, aureole radiances are hardly sensitive to particle shape and chemical composition, thus aureole radiances are well-suited for the retrieval of the size of ash and dust particles. It is expected that the accuracy of the retrievals further improves if all parameters observed by photometer are considered

MOPSMAP v1.0: a versatile tool for the modeling of aerosol optical properties

The spatiotemporal distribution and characterization of aerosol particles are usually determined by remotesensing and optical in situ measurements. These measurements are indirect with respect to microphysical properties, and thus inversion techniques are required to determine the aerosol microphysics. Scattering theory provides the link between microphysical and optical properties;it is not only needed for such inversions but also for radiative budget calculations and climate modeling. However, optical modeling can be very time-consuming, in particular if nonspherical particles or complex ensembles are involved. In this paper we present the MOPSMAP package (Modeled optical properties of ensembles of aerosol particles), which is computationally fast for optical modeling even in the case of complex aerosols. The package consists of a data set of pre-calculated optical properties of single aerosol particles, a Fortran program to calculate the properties of user-defined aerosol ensembles, and a user-friendly web interface for online calculations. Spheres, spheroids, and a small set of irregular particle shapes are considered over a wide range of sizes and refractive indices. MOPSMAP provides the fundamental optical properties assuming random particle orientation, including the scattering matrix for the selected wavelengths. Moreover, the output includes tables of frequently used properties such as the single-scattering albedo, the asymmetry parameter, or the lidar ratio. To demonstrate the wide range of possible MOPSMAP applications, a selection of examples is presented, e.g., dealing with hygroscopic growth, mixtures of absorbing and non-absorbing particles, the relevance of the size equivalence in the case of nonspherical particles, and the variability in volcanic ash microphysics. The web interface is designed to be intuitive for expert and nonexpert users. To support users a large set of default settings is available, e.g., several wavelength-dependent refractive indices, climatologically representative size distributions, and a parameterization of hygroscopic growth. Calculations are possible for single wavelengths or user-defined sets (e.g., of specific remote-sensing application). For expert users more options for the microphysics are available. Plots for immediate visualization of the results are shown. The complete output can be downloaded for further applications. All input parameters and results are stored in the user's personal folder so that calculations can easily be reproduced. The web interface is provided at https://mopsmap.net (last access: 9 July 2018) and the Fortran program including the data set is freely available for offline calculations, e.g., when large numbers of different runs for sensitivity studies are to be made

Case Study on Combined Lidar-Photometer Retrieval of Volcanic ASH Properties

We study the benefit of considering sun-/sky-photometer measurements in a microphysical lidar retrieval. Furthermore, to assess the importance of the aerosol model employed by the retrieval, we compare results obtained using a spheroid aerosol model with results using an advanced aerosol model that considers irregular particle shapes. Preliminary results are shown for the mass extinction conversion factor and the single scattering albedo during a measurement case of long-range-transported volcanic ash

Saharan dust contribution to the Caribbean summertime boundary layer - a lidar study during SALTRACE

Dual-wavelength lidar measurements with the small lidar system POLIS of the Ludwig-Maximilians-Universitat Munchen were performed during the SALTRACE experiment at Barbados in June and July 2013. Based on high-accuracy measurements of the linear depolarization ratio down to about 200m above ground level, the dust volume fraction and the dust mass concentration within the convective marine boundary layer can be derived. Additional information from radiosonde launches at the ground-based measurement site provide independent information on the convective marine boundary layer height and the meteorological situation within the convective marine boundary layer. We investigate the lidar-derived optical properties, the lidar ratio and the particle linear depolarization ratio at 355 and 532 nm and find mean values of 0.04 (SD 0.03) and 0.05 (SD 0.04) at 355 and 532 nm, respectively, for the particle linear depolarization ratio, and (26 +/- 5) sr for the lidar ratio at 355 and 532 nm. For the concentration of dust in the convective marine boundary layer we find that most values were between 20 and 50 mu g m(-3). On most days the dust contribution to total aerosol volume was about 30-40 %. Comparing the dust contribution to the column-integrated sun-photometer measurements we see a correlation between high dust contribution, high total aerosol optical depth and a low Angstrom exponent, and of low dust contribution with low total aerosol optical depth

Modelling lidar-relevant optical properties of complex mineral dust aerosols

We model lidar-relevant optical properties of mineral dust aerosols and compare the modelling results with optical properties derived from lidar measurements during the SAMUM field campaigns. The Discrete Dipole Approximation is used for optical modelling of single particles. For modelling of ensemble properties, the desert aerosol type of the OPAC aerosol dataset is extended by mixtures of absorbing and non-absorbing irregularly shaped mineral dust particles. Absorbing and non-absorbing particles are mixed to mimic the natural mineralogical inhomogeneity of dust particles. A sensitivity study reveals that the mineralogical inhomogeneity is critical for the lidar ratio at short wavelengths; it has to be considered for agreement with the observed wavelength dependence of the lidar ratio. The amount of particles with low aspect ratios (about 1.4 and lower) affects the lidar ratio at any lidar wavelength; their amount has to be low for agreement with SAMUM observations. Irregularly shaped dust particles with typical refractive indices, in general, have higher linear depolarization ratios than corresponding spheroids, and improve the agreement with the observations

In situ aerosol characterization at Cape Verde, Part 2: Parametrization of relative humidity- and wavelength-dependent aerosol optical properties

An observation-based numerical study of humidity-dependent aerosol optical properties of mixed marine and Saharan mineral dust aerosol is presented. An aerosol model was developed based on measured optical and microphysical properties to describe the marine and Saharan dust aerosol at Cape Verde. A wavelength-dependent optical equivalent imaginary part of the refractive index and a scattering non-sphericity factor for Saharan dustwere derived. Simulations of humidity effects on optical properties by the aerosol model were validated with relative measurements of the extinction coefficient at ambient conditions. Parametrizations were derived to describe the humidity dependence of the extinction, scattering, and absorption coefficients as well as the asymmetry parameter and single scattering albedo. For wavelengths (300–950 nm) and dry dust volume fractions (0–1), aerosol optical properties as a function of relative humidity (RH = 0–90%) can be calculated from tabulated parameters. For instance, at a wavelength of 550 nm, a volume fraction of 0.5 of dust on the total particle volume (dry conditions) and a RH of 90%, the enhancements for the scattering, extinction and absorption coefficients are 2.55, 2.46 and 1.04, respectively, while the enhancements for the asymmetry parameter and single scattering albedo are 1.11 and 1.04

Particle settling and vertical mixing in the Saharan Air Layer as seen from an integrated model, lidar, and in situ perspective

Long-range transport of aerosol in the Saharan Air Layer (SAL) across the Atlantic plays an important role for weather, climate, and ocean fertilization. However, processes occurring within the SAL and their effects on aerosol properties are still unclear. In this work we study particle settling and vertical mixing within the SAL based on measured and modeled vertical aerosol profiles in the upper 1 km of the transported SAL. We use ground-based lidar measurements and airborne particle counter measurements over the western Atlantic, collected during the SALTRACE campaign, as well as space-based CALIOP lidar measurements from Africa to the western Atlantic in the summer season. In our model we take account of the optical properties and the Stokes gravitational settling of irregularly shaped Saharan dust particles. We test two hypotheses about the occurrence of vertical mixing within the SAL over the Atlantic to explain the aerosol profiles observed by the lidars and the particle counter. Our first hypothesis (H1) assumes that no mixing occurs in the SAL leading to a settling-induced separation of particle sizes. The second hypothesis (H2) assumes that vertical mixing occurs in the SAL allowing large super-micron dust particles to stay airborne longer than without mixing. The uncertainties of the particle linear depolarization ratio (delta(l)) profiles measured by the ground-based lidars are comparable to the modeled differences between H1 and H2 and do not allow us to conclude which hypothesis fits better. The SALTRACE in situ data on size-resolved particle number concentrations show a presence of large particles near the SAL top that is inconsistent with H1. The analysis of the CALIOP measurements also reveals that the average delta(l) profile over the western Atlantic is inconsistent with H1. Furthermore, it was found that the average delta(l) profile in the upper 1 km of the SAL does not change along its transport path over the Atlantic. These findings give evidence that vertical mixing within the SAL is a common phenomenon with significant consequences for the evolution of the size distribution of super-micron dust particles during transport over the Atlantic. Further research is needed to precisely characterize the processes that are relevant for this phenomenon

Characterization of the planetary boundary layer during SAMUM-2 by means of lidar measurements

Measurements with two Raman-depolarization lidars of the Meteorological Institute of the Ludwig-Maximilians- Universit¨at, M¨unchen, Germany, performed during SAMUM-2, were used to characterize the planetary boundary layer (PBL) over Praia, Cape Verde. A novel approach was used to determine the volume fraction of dust υd in the PBL. This approach primarily relies on accurate measurements of the linear depolarization ratio. Comparisons with independent in situ measurements showed the reliability of this approach. Based on our retrievals, two different phases could be distinguished within the measurement period of almost one month. The first (22–31 January 2008) was characterized by high aerosol optical depth (AOD) in the PBL and large υd > 95%. During the second phase, the AOD in the PBL was considerably lower and υd less than ∼40%. These findings were in very good agreement with ground based in situ measurements, when ambient volume fractions are considered that were calculated from the actual measurements of the dry volume fraction. Only in cases when dust was not the dominating aerosol component (second phase), effects due to hygroscopic growth became important

Determination of complex refractive indices and optical properties of volcanic ashes in the thermal infrared based on generic petrological compositions

The spaceborne detection of volcanic ash clouds at infrared wavelengths helps to avoid regions with enhanced volcanic ash concentrations that pose a threat to aviation. Current volcanic ash data retrievals require detailed information on microphysical properties and the refractive index of volcanic ash, which are highly variable. Uncertainties in the latter currently limit the quality of volcanic ash nowcasts. Here, we introduce a novel method to calculate the complex refractive indices of volcanic ashes at wavelengths from 5 to 15 μm from measurements of their individual components based on generic petrological ash compositions. Thereby the refractive indices for volcanic glasses and bulk volcanic ashes of different chemical compositions are derived. The variability of the latter is mainly influenced by the silica content and the porosity and to a minor degree by the glass-to-crystals ratio. Calculating optical properties exhibits an equally large impact of bulk composition and grain size distribution, whereas particle shape is considered less important for particle sizes of the order 1 μm. Using these optical properties to determine brightness temperature differences between the 11 μm and 12 μm channels we show that the effect of ash composition is non-negligible for modern satellite instruments. Particularly, the dependence of the volcanic ash on the silica content (and to a much smaller extent on the glass-to-crystals ratio) is observable in its refractive index, its optical properties and the brightness temperature difference, indicating that composition might be retrievable to some degree by remote sensing methods